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Highly stable and tunable peptoid/hemin enzymatic mimetics with natural peroxidase-like activities

Tengyue Jian, Yicheng Zhou, Peipei Wang, Wenchao Yang, Peng Mu, Xin Zhang, Xiao Zhang, Chun‐Long Chen

2022Nature Communications94 citationsDOIOpen Access PDF

Abstract

Abstract Developing tunable and stable peroxidase mimetics with high catalytic efficiency provides a promising opportunity to improve and expand enzymatic catalysis in lignin depolymerization. A class of peptoid-based peroxidase mimetics with tunable catalytic activity and high stability is developed by constructing peptoids and hemins into self-assembled crystalline nanomaterials. By varying peptoid side chain chemistry to tailor the microenvironment of active sites, these self-assembled peptoid/hemin nanomaterials (Pep/hemin) exhibit highly modulable catalytic activities toward two lignin model substrates 2,2-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) and 3,3’,5,5’-tetramethylbenzidine. Among them, a Pep/hemin complex containing the pyridyl side chain showed the best catalytic efficiency ( V max / K m = 5.81 × 10 −3 s −1 ). These Pep/hemin catalysts are highly stable; kinetics studies suggest that they follow a peroxidase-like mechanism. Moreover, they exhibit a high efficacy on depolymerization of a biorefinery lignin. Because Pep/hemin catalysts are highly robust and tunable, we expect that they offer tremendous opportunities for lignin valorization to high value products.

Topics & Concepts

HeminDepolymerizationChemistryCatalysisLigninPeroxidasePeptoidCombinatorial chemistryNanomaterialsOrganic chemistryEnzymePeptideNanotechnologyBiochemistryMaterials scienceHemeChemical Synthesis and AnalysisEnzyme-mediated dye degradationSulfur-Based Synthesis Techniques